Mass spectrometry measurements show the formation of highly superhydrogenated derivatives of the polycyclic aromatic hydrocarbon molecule coronene through H atom addition reactions. The observed product mass distribution provides evidence also for abstraction reactions resulting in H2 formation, in agreement with recent IR measurements. Complementary density functional theory calculations confirm the stability of the observed superhydrogenated species toward spontaneous H and H2 loss indicating that abstraction reactions may be the dominant route to H2 formation involving neutral polycyclic aromatic hydrocarbons (PAHs). The results indicate that highly superhydrogenated PAHs could well be formed and could act as efficient catalysts for H2 formation in the interstellar medium in low UV flux regions. © 2012. The American Astronomical Society. All rights reserved..